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1、CatalysisLetters43(1997)107-115107Characterisationoftheactivephaseincaesium-dopediron-vanadium•oxidecatalystsfortheselectiveoxidationofpolyaromaticsAndrewP.E.Yorka,*,AngelikaBrucknera,Peter-MichaelWildeb,HartmutMehnerc,MartinKraumdandManfredBaernsd,taInstitutfUrangewandteChemieBerlin-A
2、dlershofe.V.,RudowerChaussee5,D-l2484Berlin,GermanybGesellschaftzurForderungangewandteOptik,OptoelektronikundSpektroskopie(GOS),RudowerChaussee5,D-l2484Berlin,GermanyCBundesanstaltfiirMaterial/orschungund-priifung,RudowerChaussee5,D-l2484Berlin,GermanydRuhr-UniversitiitBochum,Lehrstuhl
3、fiirTechnischeChemie,D-44780Bochum,GermanyReceived22July1996;accepted29October1996Theadditionofcaesiumsulphatetounsupportedvanadium-iron-oxidematerialsleadstotheformationofanamorphousnon-stoichiometricphase,aswellasthecrystallinephases,FeVO.,Fe2V.013,andFel_XS(pyrrhotite).Caesiumwasonl
4、ypresentintheamorphouspartsofthesample,andtheamountofthenewphaseformedwasfoundtovarydependingonthevanadium:ironratioandtheamountofcaesiumdopantadded.ThenewphasecontainsFe3+ionswithoxidelatticevacanciesintheircoordinationsphere,i.e.Fe3+-VoCe-)species.Catalytictestingdemonstratedthatthec
5、aesium-dopedsamplesweremoreselectivefortheoxida•tionoffluoreneto9-fluorenone.Theroleofthecaesiumisprobablytomodifythesurfaceacidityofthecatalystandactintheforma•tionofstableoxidelatticevacancies.Keywords:selectiveoxidation,polyaromatics,Cs-dopcdironvanadates,ironsulphide31.Introduction
6、anFe+cationlocatedincloseproximitytoanoxygen3vacancyoccupiedbyanelectron,i.e.Fe+-Vo{e-)spe•Theselectiveoxidationofpolyaromatics(e.g.anthra•cies;thesespecieshavealsobeenobservedinotheroxidiccene,fluorene)toketonesandanhydridesisofconsider•systems,suchasiron-dopedBaTi03[9].Itwasproposeda
7、bleindustrialandacademicinterest,andvariousthatthisnewphasewasimportantintheimprovedselec•vanadium-oxide-basedcatalystshavebeenusedfortivitiesobserved.thesereactions[1].Forexample,Majunkeetal.studiedDespitethisearlierwork,themorphologyofthecae•theoxidationoffluoreneoverunsupportedvan
